Resonance-Activated Spin-Flipping for Efficient Organic Ultralong Room-Temperature Phosphorescence

Triplet-excited-state-involved photonic and electronic properties have attracted tremendous attention for next-generation technologies. To populate triplet states, facile intersystem crossing (ISC) for efficient exciton spin-flipping is crucial, but it remains challenging in organic molecules free of heavy atoms. Here, a new strategy is proposed to enhance the ISC of purely organic optoelectronic molecules using heteroatom-mediated resonance structures capable of promoting spin-flipping at large singlet–triplet splitting energies with the aid of the fluctuation of the state energy and n-orbital component upon self-adaptive resonance variation. Combined experimental and theoretical investigations confirm the key contributions of the resonance variation to the profoundly promoted spin-flipping with ISC rate up to ≈10⁷ s⁻¹ in the rationally designed NPX (X = O or S) resonance molecules. Importantly, efficient organic ultralong room-temperature phosphorescence (OURTP) with simultaneously elongated lifetime and improved efficiency results overcoming the intrinsic competition between the OURTP lifetime and efficiency. With the spectacular resonance-activated OURTP molecules, time-resolved and color-coded quick response code devices with multiple information encryptions are realized, demonstrating the fundamental significance of this approach in boosting ISC dynamically for advanced optoelectronic applications.